First-principles study on the thermal stability of LiNiO2 materials coated by amorphous Al2O3 with atomic layer thickness

Joonhee Kang, Byungchan Han

Research output: Contribution to journalArticle

23 Citations (Scopus)

Abstract

Using first-principles calculations, we study how to enhance thermal stability of high Ni compositional cathodes in Li-ion battery application. Using the archetype material LiNiO2 (LNO), we identify that ultrathin coating of Al2O3 (0001) on LNO(012) surface, which is the Li de-/intercalation channel, substantially improves the instability problem. Density functional theory calculations indicate that the Al2O3 deposits show phase transition from the corundum-type crystalline (c-Al2O3) to amorphous (a-Al2O3) structures as the number of coating layers reaches three. Ab initio molecular dynamic simulations on the LNO(012) surface coated by a-Al2O3 (about 0.88 nm) with three atomic layers oxygen gas evolution is strongly suppressed at T = 400 K. We find that the underlying mechanism is the strong contacting force at the interface between LNO(012) and Al2O3 deposits, which, in turn, originated from highly ionic chemical bonding of Al and O at the interface. Furthermore, we identify that thermodynamic stability of the a-Al2O3 is even more enhanced with Li in the layer, implying that the protection for the LNO(012) surface by the coating layer is meaningful over the charging process. Our approach contributes to the design of innovative cathode materials with not only high-energy capacity but also long-term thermal and electrochemical stability applicable for a variety of electrochemical energy devices including Li-ion batteries.

Original languageEnglish
Pages (from-to)11599-11603
Number of pages5
JournalACS Applied Materials and Interfaces
Volume7
Issue number21
DOIs
Publication statusPublished - 2015 Jun 3

Fingerprint

Coated materials
Thermodynamic stability
Coatings
Cathodes
Deposits
Corundum
Aluminum Oxide
Intercalation
Density functional theory
Molecular dynamics
Gases
Phase transitions
Oxygen
Crystalline materials
Computer simulation
Lithium-ion batteries

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

Cite this

@article{c0f37a80ab5f4532893563d69f547c66,
title = "First-principles study on the thermal stability of LiNiO2 materials coated by amorphous Al2O3 with atomic layer thickness",
abstract = "Using first-principles calculations, we study how to enhance thermal stability of high Ni compositional cathodes in Li-ion battery application. Using the archetype material LiNiO2 (LNO), we identify that ultrathin coating of Al2O3 (0001) on LNO(012) surface, which is the Li de-/intercalation channel, substantially improves the instability problem. Density functional theory calculations indicate that the Al2O3 deposits show phase transition from the corundum-type crystalline (c-Al2O3) to amorphous (a-Al2O3) structures as the number of coating layers reaches three. Ab initio molecular dynamic simulations on the LNO(012) surface coated by a-Al2O3 (about 0.88 nm) with three atomic layers oxygen gas evolution is strongly suppressed at T = 400 K. We find that the underlying mechanism is the strong contacting force at the interface between LNO(012) and Al2O3 deposits, which, in turn, originated from highly ionic chemical bonding of Al and O at the interface. Furthermore, we identify that thermodynamic stability of the a-Al2O3 is even more enhanced with Li in the layer, implying that the protection for the LNO(012) surface by the coating layer is meaningful over the charging process. Our approach contributes to the design of innovative cathode materials with not only high-energy capacity but also long-term thermal and electrochemical stability applicable for a variety of electrochemical energy devices including Li-ion batteries.",
author = "Joonhee Kang and Byungchan Han",
year = "2015",
month = "6",
day = "3",
doi = "10.1021/acsami.5b02572",
language = "English",
volume = "7",
pages = "11599--11603",
journal = "ACS applied materials & interfaces",
issn = "1944-8244",
publisher = "American Chemical Society",
number = "21",

}

First-principles study on the thermal stability of LiNiO2 materials coated by amorphous Al2O3 with atomic layer thickness. / Kang, Joonhee; Han, Byungchan.

In: ACS Applied Materials and Interfaces, Vol. 7, No. 21, 03.06.2015, p. 11599-11603.

Research output: Contribution to journalArticle

TY - JOUR

T1 - First-principles study on the thermal stability of LiNiO2 materials coated by amorphous Al2O3 with atomic layer thickness

AU - Kang, Joonhee

AU - Han, Byungchan

PY - 2015/6/3

Y1 - 2015/6/3

N2 - Using first-principles calculations, we study how to enhance thermal stability of high Ni compositional cathodes in Li-ion battery application. Using the archetype material LiNiO2 (LNO), we identify that ultrathin coating of Al2O3 (0001) on LNO(012) surface, which is the Li de-/intercalation channel, substantially improves the instability problem. Density functional theory calculations indicate that the Al2O3 deposits show phase transition from the corundum-type crystalline (c-Al2O3) to amorphous (a-Al2O3) structures as the number of coating layers reaches three. Ab initio molecular dynamic simulations on the LNO(012) surface coated by a-Al2O3 (about 0.88 nm) with three atomic layers oxygen gas evolution is strongly suppressed at T = 400 K. We find that the underlying mechanism is the strong contacting force at the interface between LNO(012) and Al2O3 deposits, which, in turn, originated from highly ionic chemical bonding of Al and O at the interface. Furthermore, we identify that thermodynamic stability of the a-Al2O3 is even more enhanced with Li in the layer, implying that the protection for the LNO(012) surface by the coating layer is meaningful over the charging process. Our approach contributes to the design of innovative cathode materials with not only high-energy capacity but also long-term thermal and electrochemical stability applicable for a variety of electrochemical energy devices including Li-ion batteries.

AB - Using first-principles calculations, we study how to enhance thermal stability of high Ni compositional cathodes in Li-ion battery application. Using the archetype material LiNiO2 (LNO), we identify that ultrathin coating of Al2O3 (0001) on LNO(012) surface, which is the Li de-/intercalation channel, substantially improves the instability problem. Density functional theory calculations indicate that the Al2O3 deposits show phase transition from the corundum-type crystalline (c-Al2O3) to amorphous (a-Al2O3) structures as the number of coating layers reaches three. Ab initio molecular dynamic simulations on the LNO(012) surface coated by a-Al2O3 (about 0.88 nm) with three atomic layers oxygen gas evolution is strongly suppressed at T = 400 K. We find that the underlying mechanism is the strong contacting force at the interface between LNO(012) and Al2O3 deposits, which, in turn, originated from highly ionic chemical bonding of Al and O at the interface. Furthermore, we identify that thermodynamic stability of the a-Al2O3 is even more enhanced with Li in the layer, implying that the protection for the LNO(012) surface by the coating layer is meaningful over the charging process. Our approach contributes to the design of innovative cathode materials with not only high-energy capacity but also long-term thermal and electrochemical stability applicable for a variety of electrochemical energy devices including Li-ion batteries.

UR - http://www.scopus.com/inward/record.url?scp=84930681864&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84930681864&partnerID=8YFLogxK

U2 - 10.1021/acsami.5b02572

DO - 10.1021/acsami.5b02572

M3 - Article

VL - 7

SP - 11599

EP - 11603

JO - ACS applied materials & interfaces

JF - ACS applied materials & interfaces

SN - 1944-8244

IS - 21

ER -